AbstractWe report the possibility of recycling carbonaceous materials (GC) from used/spent Li‐ion batteries (LIBs) and re‐using the material again as a negative electrode. In addition to LIB, the possibility of using them in Li‐ion capacitor (LIC) configuration with activated carbon is also explored. First, the carbonaceous materials are recovered from the mechanical treatment and subsequent leaching process. After the successful recovery, the Li‐insertion properties are studied in half‐cell assembly and it exhibits very decent electrochemical activity. While re‐using GC as an anode, large irreversibility is noted compared to fresh usage. Therefore, the elimination of such irreversible capacity is desperately required prior to the fabrication of either LIBs or LICs. Full‐cell LIB is assembled with olivine phase LiFePO4 cathode and the configuration delivers a maximum energy density of ∼313 Wh kg−1. Similarly, the GC is used as an anode in LIC assembly with commercial activated carbon. The LIC displays an energy density of ∼112 Wh kg−1 with decent cycling profiles.